Process for normalizing the concentration of analytes in a urine sample

ABSTRACT

Process for normalizing the concentration of at least one analyte in a urine sample, comprising the following steps:
     a) determining the concentration of at least one analyte;   b) determining the concentration of at least one collagen or collagen fragment;   c) normalizing the concentration of said at least one analyte relative to the concentration of said at least one collagen or collagen fragment.

RELATED APPLICATION

This application is a continuation of U.S. patent application Ser. No.12/530,029, which is a national stage filing of PCT Application No.PCT/EP2008/052730 filed Mar. 6, 2008, which claims priority of EuropeanPatent Application No. 07103684.2 filed Mar. 7, 2007, all of which arehereby incorporated herein by reference.

TECHNICAL FIELD OF THE INVENTION

The present invention relates to a process for normalizing theconcentration of analytes in a urine sample.

BACKGROUND OF THE INVENTION

Urine samples have been used for medical laboratory examinations for along time. Urine samples contain a variety of substances that areinteresting under medical aspects, for example, degradation products ofmedicaments or illegal drugs, hormones, pathogens, proteins etc.

While often (only) the total protein content was recurred to forevaluating a urine sample in the past, it is recognized more and morethat the composition of the proteins in urine, in particular, alsocontains relevant medical information.

WO 01/84140 and WO 2004/068130 describe Processes and devices fordetermining protein and peptide patterns in a liquid sample, forexample, a urine sample.

WO 2005/024409 describes devices and processes for the quantitativeevaluation of the polypeptides contained in a sample of body fluids andmarkers for recognizing pathological conditions. For example, it isshown how different diseases are associated with the occurrence ofdifferent polypeptide markers. It is observed that differentpolypeptides occur more or less frequently in certain diseases ascompared to healthy patients.

WO 2006/106129 among others describes so-called amplitude markers inwhich two states, for example states of health and disease, aredistinguished from one another, not by the occurrence, but by theamplitude, i.e., the concentration, of the markers in the sample. Inorder to compensate for different protein concentrations of differentsamples, the overall amplitude is normalized to 1 million counts afteran examination of the sample by mass spectrometry in WO 2006/106129.

SUMMARY OF THE INVENTION

However, there is still a need for more specific normalizationprocedures for comparing different concentrations of analytes in thesample and therefore achieve a better comparability between thereference samples and measured samples.

Surprisingly, this object can be achieved by a process for normalizingthe concentration of at least one analyte in a urine sample, comprisingthe following steps:

a) determining the concentration of at least one analyte;b) determining the concentration of at least one collagen or collagenfragment;c) normalizing the concentration of said at least one analyte relativeto the concentration of said at least one collagen or collagen fragment.

BRIEF DESCRIPTION OF THE DRAWINGS

FIG. 1 depicts the regression plot of five protein standards for Example2.

FIG. 2 depicts the normalization of the collagen fragments in Example 3.

FIG. 3 is a table listing collagen fragments and their sequences.

DESCRIPTION OF THE INVENTION

The process according to the invention has a wide variety ofapplications.

First, the content of analytes, collagen or collagen fragments isdetermined. For the determination, for example, UV/Vis detectors,fluorescence detectors, refractive index detectors, diode arraydetectors, mass spectrometers, gel scanners, the staining of theproteins, for example, with Coomassie brilliant blue, silver staining,Cy2, Cy3, Cy5 or the like, or the derivatization, for example, withITRAC (isotope tags for relative and absolute qualification) and ICAT(isotope coded affinity tagging) followed by detection of thederivatized peptides may be used.

According to the invention, collagen or collagen fragments are employedfor normalizing the samples. At least one collagen or collagen fragmentis identified in the sample. For this purpose, identification bymigration and retention times, in particular, optionally completed bymass spectra, UV/Vis spectra, fluorescence spectra or the affinity forparticular ligands, for example, specific antibodies, is suitable.

The concentration of the analyte can then be normalized to theconcentration of said at least one collagen or collagen fragment, i.e.,the concentrations of analytes are measured relative to theconcentration of the reference collagen or collagen fragments.

Preferably, however, not one collagen or collagen fragment, but several,for example, two or three or four or five or 10, 20, 30, 40 or 50collagens or collagen fragments are employed for normalization.

In a preferred embodiment, the analyte does not comprise anyhydroxypyridinium collagen cross-links, especially nohydroxylysylpyridinoline (Pyd) and deoxypyridinoline (Dpd). Preferably,none of these compounds is employed for normalizing the concentration ofanother analyte either.

Preferably used collagen fragments are stated in the following Table:

Seq. Swissprot Accession Calc. mass ID No. Protein name name number [M]1 Collagen alpha-1 (I) chain [777-787] [Homo sapiens] CO1A1 Humangi115269 1016.441 2 Collagen alpha-1 (I) chain [546-558] [Homo sapiens]CO1A1 Human gi115269 1194.552 3 Collagen alpha-1 (I) chain [798-810][Homo sapiens] CO1A1 Human gi115269 1250.553 4 Collagen alpha-1 (I)chain [546-559] [Homo sapiens] CO1A1 Human gi115269 1265.589 5 Collagenalpha-1 (III) chain [796-808] [Homo sapiens] CO3A1 Human gi1153061268.563 6 Collagen alpha-1 (II) chain [511-524] [Homo sapiens] CO2A1Human gi115287 1378.611 7 Collagen alpha-1 (I) chain [543-558] [Homosapiens] CO1A1 Human gi115269 1435.658 8 Collagen alpha-1 (III) chain[642-657] [Homo sapiens] CO3A1 Human gi115306 1438.669 9 Collagenalpha-1 (I) chain [543-558] [Homo sapiens] CO1A1 Human gi115269 1451.65310 Collagen alpha-1 (I) chain [542-558] [Homo sapiens] CO1A1 Humangi115269 1508.674 11 Collagen alpha-1 (XV) chain [1093-1109] [Homosapiens] COFA1 Human gi68839886 1523.726 12 Collagen alpha-1 (I) chain[543-560] [Homo sapiens] CO1A1 Human gi115269 1579.711 13 Collagenalpha-1 (III) chain [587-604] [Homo sapiens] CO3A1 Human gi1153061623.724 14 Collagen alpha-1 (I) chain [541-560] [Homo sapiens] CO1A1Human gi115269 1737.781 15 Collagen alpha-1 (III) chain [642-661] [Homosapiens] CO3A1 Human gi115306 1834.833 16 Collagen alpha-1 (III) chain[1174-1195] [Homo sapiens] CO3A1 Human gi115306 2025.866 17 Collagenalpha-1 (I) chain [648-669] [Homo sapiens] CO1A1 Human gi115269 2046.94918 Collagen alpha-1 (I) chain [229-249] [Homo sapiens] CO1A1 Humangi115269 2063.926 19 Collagen alpha-1 (III) chain [586-604] [Homosapiens] CO3A1 Human gi115306 2078.925 20 Collagen alpha-1 (I) chain[647-669] [Homo sapiens] CO1A1 Human gi115269 2087.976 21 Collagenalpha-1 (I) chain [647-669] [Homo sapiens] CO1A1 Human gi115269 2103.97122 Collagen alpha-1 (I) chain [646-669] [Homo sapiens] CO1A1 Humangi115269 2159.013 23 Collagen alpha-1 (I) chain [432-455] [Homo sapiens]CO1A1 Human gi115269 2169.977 24 Collagen alpha-1 (I) chain [646-669][Homo sapiens] CO1A1 Human gi115269 2175.008 25 Collagen alpha-1 (I)chain [819-843] [Homo sapiens] CO1A1 Human gi115269 2220.988 26 Collagenalpha-1 (I) chain [431-455] [Homo sapiens] CO1A1 Human gi115269 2226.99927 Collagen alpha-1 (I) chain [699-725] [Homo sapiens] CO1A1 Humangi115269 2281.979 28 Collagen alpha-1 (I) chain [819-844] [Homo sapiens]CO1A1 Human gi115269 2292.025 29 Collagen alpha-1 (III) chain [813-840][Homo sapiens] CO3A1 Human gi115306 2564.149 30 Collagen alpha-1 (III)chain [1168-1195] [Homo sapiens] CO3A1 Human gi115306 2679.202 31Collagen alpha-1 (III) chain [1168-1195] [Homo sapiens] CO3A1 Humangi115306 2695.197 32 Collagen alpha-1 (III) chain [610-639] [Homosapiens] CO3A1 Human gi115306 2742.248 33 Collagen alpha-1 (III) chain[448-477] [Homo sapiens] CO3A1 Human gi115306 2825.270 34 Collagenalpha-1 (I) chain [1011-1041] [Homo sapiens] CO1A1 Human gi1152692942.299 35 Collagen alpha-1 (I) chain [537-569] [Homo sapiens] CO1A1Human gi115269 3011.386 36 Collagen alpha-1 (I) chain [1011-1040] [Homosapiens] CO1A1 Human gi115269 3013.336 37 Collagen alpha-2 (I) chain[830-865] [Homo sapiens] CO1A2 Human gi82654930 3248.533 38 Collagenalpha-1 (I) chain [1007-1041] [Homo sapiens] CO1A1 Human gi1152693266.442 39 Collagen alpha-1 (III) chain [910-948] [Homo sapiens] CO3A1Human gi115306 3441.603 40 Collagen alpha-1 (I) chain [630-674] [Homosapiens] CO1A1 Human gi115269 4169.916 41 Collagen alpha-1 (III) chain[319-366] [Homo sapiens] CO3A1 Human gi115306 4289.919 42 Collagenalpha-1 (III) chain [319-366] [Homo sapiens] CO3A1 Human gi1153064305.914The sequences are given in FIG. 3.

The invention also relates to the use of collagen fragments fornormalizing the analyte concentration of urine samples, especially withthe collagen fragments as described above.

Preferred analytes whose contents are to be normalized include, inparticular, proteins, peptides, lipids, metabolites, salts and otherionic compounds, carbohydrates.

The use of the process for normalizing peptide concentrations isparticularly preferred.

In one embodiment, the sample is first subdivided into subsamples.

Different methods may be employed to achieve this, for example:

-   -   chromatographic methods, such as affinity chromatography,        ion-exchange chromatography, reversed-phase chromatography,        hydrophobic interaction chromatography, gel filtration,        optionally using FPLC or HPLC;    -   adsorption to specific materials, such as SELDI process,        ClinProt process;    -   electrophoretic methods, such as gel electrophoresis or        capillary electrophoresis.

The invention is further illustrated by the following Examples:

EXAMPLES Example 1

A urine sample was examined by means of HPLC with a downstream diodearray detector (DAD). The raw date are stated in the Table. Peaks wereidentified by means of the retention time and spectra in the DAD. Themeasurement was compared with previously determined standards for thesefour collagen fragments, and a conversion factor was calculated foreach. The average of these factors (0.80761277 in this case) wasemployed as a normalizing factor for all the other signals. Thenormalized signals are stated in the last column.

Peak Normalizing Normalized No. Signal Standard factor signal intensity1 126.8033157 157.0100429 2 146.5503894 181.4612086 3 3115.5198754073.54509 0.76481782 3857.690207 4 590.1256269 730.7036846 55461.634925 6762.690148 6 150.3823428 186.2059991 7 39.178082748.51097474 8 8.5271778 10.55849798 9 394.6322538 488.6404331 1050.0342319 61.9532451 11 1577.919488 1953.807005 12 539.3141163667.7879996 13 400.4296182 495.8188292 14 8.8306578 10.93427212 15148.7699163 184.209465 16 538.5410307 666.8307518 17 1389.8609451720.949688 18 93.4206021 115.6749937 19 1024.846846 1276.567820.80281426 1268.982963 20 2344.443075 2902.929673 21 435.1965894538.86789 22 114.2890587 141.514675 23 15.9397308 19.73684839 248.9629632 11.09809494 25 398.4975981 493.4265688 26 6940.8252 8643.258760.80303337 8594.248947 27 76.7856591 95.07732162 28 61.261849875.85547438 29 64.5422931 79.9173756 30 559.1427462 692.3401497 31323.2918818 400.3055594 32 14.1058476 17.46610272 33 399.1654701494.2535393 34 4612.278375 5711.002284 35 174.3985782 215.9433142 36136.4525784 168.9579257 37 909.9711288 1126.741877 38 62.172219676.9827099 39 119.8605303 148.4133668 40 2922.828975 3399.485710.85978563 3619.097026 41 2.625588 3.251048147 42 52.8236532 65.4071544543 178.5294621 221.0582456 0.80761277

Example 2

A urine sample was separated by means of 2D electrophoresis as describedin Thong-boonkerd et al. in Kidney Int 62: 1461-1469 (2002), over a pHrange of from 3 to 10 and using a 10% polyacrylamide gel having a lengthof 22 cm. The gel was stained with Coomassie stain, and the collagenswere detected in a gel prepared in parallel by means of immunologicalmethods (Western blot). Predetermined standards for these five proteinswere employed, and a linear regression performed. With this calibrationformula, the further values were converted. The formula wasY=103.82x−127449. The R² value was 0.957.

Peak Normalized No. Signal Standard signal intensity 1 4508518.988467946992.3 2 153935103 15981414944 3 23582568 2448214761 4 44251661.94594080090 5 586248.746 60736895.81 6 948640.866 98360445.71 71383514.774 143509054.8 8 122812941 12750312086 9 2944789.572305600604.4 10 30550952.65 3171672456 11 1089289.56 117284244.8112962593.1 12 577112.586 59788379.68 13 1130932.024 117285913.7 14913664.024 94729149.97 15 397773.048 41169348.84 16 6931703.714719522030.6 17 38342270.25 3980567048 18 2391089.672 248115480.7 192250316.422 233500401.9 20 932726.014 96708165.77 21 10695075.821110235323 22 1438795.038 149248251.8 23 8548926.298 887422079.3 247982762.024 828642904.3 25 519540.4375 58011688.21 53811239.22 264877082.25 506211230.2 27 27564764.65 2861646417 28 20622151.952140864367 29 3862566.202 400884174.1 30 219714.4865 23759647.5822683308.99 31 13240495.55 1374500799 32 6102716.5 633456578 333523566.41 365689215.7 34 1011312.708 104867036.3 35 10681983.251108876052 36 390792.574 40444636.03 37 3552944.744 368739274.3 388037397.154 834315123.5 39 1966378.988 204022017.5 40 89404658.259281864171 41 2051887.75 212899537.2 42 7424138.214 770646580.4 4332377626.4 3361317724 44 34631829 3595349038 45 1948609.006 202177138 46107055624.3 11114387461 47 10008414.75 1038946170 48 3575878.756371120283.4 49 1359764.006 141043250.1 50 631532.685 52349499.1765438274.36 51 1981878.154 205631140.9 52 6658241.834 691131218.2 538132593.25 844198382.2 54 5853332.798 607565562.1 55 10995087.21141382504 56 3309612.762 343476548 57 5692416.786 590859261.7 583166113.976 328578504 59 20333775.95 2110925170 60 32900793.653415632948 61 5041336.916 523264149.6 62 2926167.976 303667310.3 6310445490.05 1084323328 64 775850.282 80421327.28 65 339214.04435089753.05 66 41363211.15 4294201133 67 23456220.45 2435097358 6815788615 1639046560 69 34321605.15 3563141598 70 897196.084 93019448.4471 327241.543 37343483.31 33846767.99 72 9414104.178 977244846.8 731965153.274 203894763.9 74 45057999.65 4677794075 75 877939.96891020278.48 76 3120269.268 323818906.4 77 3584994.964 372066728.2 7810224568.98 1061387302 79 735893.154 76272978.25 80 5907069.334613144489.3 81 36156493.15 3753639670 82 10877155.98 1129138884 838374707.928 869334728.1 84 16689498.2 1732576254 85 5895062.464611897936 86 1706771.568 177069575.2

The quality of the regression is shown in FIG. 1.

Example 3

A urine sample was examined by capillary electrophoresis coupled withmass spectrometry. Twenty-seven collagen fragments could be identifiedthereby, which were then compared with previously determined standards.This was followed by normalization by means of linear regression withthe proviso that the straight line must go through the value zero.Corresponding measuring data and the calibration are shown in thefollowing Table.

CE time Normalized No. (min) Mass Signal Standard signal intensity 119.948 17266.043 184882.922 1368.13362 2 19.944 17119.789 587371.1884346.54679 3 19.931 17062.977 240560 1780.144 4 19.946 16972.203352392.875 2607.70728 5 19.908 16952.465 197797.906 1463.7045 6 19.93116918.75 2107725.75 15597.1706 7 19.873 16806.326 124057.313 918.0241168 19.917 16771.715 1365796.63 10106.895 9 22.387 10342.543 119401.375883.570175 10 20.699 9905.148 89822.563 664.686966 11 20.727 9867.076526946.5 3899.4041 12 20.599 9626.376 176806.484 1308.36798 13 20.9048875.947 124966.711 924.753661 14 20.927 8837.85 796843.125 5896.6391315 19.926 8578.571 17265.779 127.766765 16 20.156 8289.725 286028.7812116.61298 17 20.078 8176.791 674227.938 4989.28674 18 57.332 6788.82438.533 3.2451442 19 19.251 6491.179 95395.688 705.928091 20 23.8656329.103 62460.586 462.208336 21 19.542 6308.096 23674.088 175.188251 2220.842 6237.104 134147.797 992.693698 23 23.72 6225.298 67887.742502.369291 24 23.66 6208.243 85896.305 635.632657 25 23.741 6186.583288461.313 2134.61372 26 23.643 6170.012 399146.313 2953.68272 27 19.6625861.38 218662.969 1618.10597 28 22.258 5635.462 14248.398 105.438145 2922.266 5612.497 112633.008 833.484259 30 22.301 5574.535 988766.1887316.86979 31 20.377 5118.564 18909.668 139.931543 32 20.441 5096.63193874.516 694.671418 33 20.448 5058.56 250174.453 1851.29095 34 23.7375039.495 283460.031 2097.60423 35 22.982 5038.431 174797.016 1293.4979236 20.431 5036.265 628288.625 4649.33583 37 23.001 5023.362 43507.188321.953191 38 20.438 5020.505 641471.938 4746.89234 39 23.009 5000.172753943.563 5579.18237 40 20.45 4998.592 2524795 18683.483 41 20.4094982.02 313462.719 2319.62412 42 20.549 4976.683 1167032.75 8636.0423543 52.301 4964.782 358.613 2.6537362 44 20.466 4960.742 14400323106562.39 45 20.358 4933.646 23247.875 1652.03428 46 22.651 4876.40451850.109 383.690807 47 38.197 4861.141 494.304 3.6578496 48 22.6824838.021 281694.156 2084.53675 49 22.655 4822.251 52409.906 387.83330450 22.683 4800.063 1058541.25 7833.20525 51 48.573 4793.838 282.4852.090389 52 55.222 4777.634 374.187 2.7689838 53 39.763 4774.006 532.923.943608 54 48.826 4772.17 272.009 2.0128666 55 57.032 4766.609 339.3832.5114342 56 19.62 4730.656 24256.555 179.498507 57 37.899 4719.6362192.44 16.224056 58 23.902 4692.252 68363.453 505.889552 59 54.4644690.256 358.075 2.649755 60 22.332 4671.967 96398.766 713.350868 6125.889 4668.661 32946.504 243.80413 62 21.078 4656.171 37012.164273.890014 63 23.915 4654.204 252635.781 1869.50478 64 19.366 4651.778422.893 3.1294082 65 25.936 4630.038 76921.227 569.21708 66 54.5674620.673 895.427 6.6261598 67 23.396 4619.578 16829.051 124.534977 6852.701 4602.985 298.8 2.21112 69 58.14 4602.554 423.734 3.1356316 7057.637 4594.426 391.032 2.8936368 71 52.603 4577.292 340.97 2.523178 7220.741 4566.496 232446.344 1720.10295 73 49.024 4560.303 642.9824.7580668 74 54.011 4559.723 4928.111 36.4680214 75 18.86 4552.372345.112 2.5538288 76 51.846 4548.482 373.052 2.7605848 77 26.0664547.384 12106.5 89.5881 78 51.365 4544.345 1851.577 13.7016698 7953.986 4543.723 22582.416 167.109878 80 54.024 4520.931 4122.54730.5068478 81 40.87 4520.884 552.198 4.0862652 82 25.763 4468.20633454.656 247.564454 83 25.839 4452.583 21824.857 161.503942 84 48.9764445.646 571.726 4.2307724 85 20.501 4443.026 18179.678 134.529617 8627.642 4439.813 97056.883 718.220934 87 24.137 4436.181 404617.5312994.16973 88 58.694 4420.792 432.338 3.1993012 89 25.813 4414.27315183.697 112.359358 90 19.965 4410.955 338675.063 2506.19547 91 20.5154405.046 291842.344 2159.63335 92 25.558 4404.052 42032.641 311.04154393 20.055 4391.25 224259.906 1659.5233 94 59.551 4390.04 363.2512.6880574 95 59.07 4383.307 677.349 5.0123826 96 20.018 4375.046105928.648 783.871995 97 25.571 4366.142 216682.813 1603.45282 98 20.0664353.102 1819283.25 13462.6961 99 22.383 4349.45 216404.641 1601.39434100 25.569 4344.106 288232.313 2132.91912 101 20.337 4334.652 45377.477335.79333 102 25.603 4328.157 542624 4015.4176 103 60.458 4319.592330.163 2.4432062 104 27.298 4307.342 30545.982 226.040267 105 25.6144306.212 529838.313 3100.93516 3920.80352 106 18.866 4302.308 277.2522.0516648 107 25.618 4290.197 708976.625 3872.09443 5246.42703 108 25.584274.179 57546.574 425.844648 109 25.607 4252.228 98721.375 730.538175110 23.903 4239.119 31304.807 231.655572 111 20.202 4233.57 31109.875230.213075 112 25.741 4229.222 27980.471 207.055485 113 23.93 4217.721698545.563 5169.23717 114 28.392 4208.093 85557.367 633.124516 11520.629 4196.917 227998.453 1687.18855 116 28.393 4192.087 152065.6881125.28609 117 27.019 4180.957 29489.236 218.220346 118 28.396 4170.166176045.016 1291.45231 1302.73312 119 23.8 4160.604 154588.094 1143.9519120 22.532 4160.021 318391.75 2356.09895 121 27.033 4160.011 69551.938514.684341 122 28.349 4154.089 35176.504 260.30613 123 27.009 4144.03562706.73 464.029802 124 22.513 4144.034 67626.914 500.439164 125 23.2944135.927 40501.199 299.708873 126 22.526 4122.078 1111014.88 8221.51008127 27.052 4121.97 143200.75 1059.68555 128 26.993 4106.017 56078.742414.982691 129 20.242 4105.763 27811.58 205.805692 130 28.055 4102.56318823.371 139.292945 131 27.022 4084.008 103050.93 762.576882 132 28.0574082.969 35312.172 261.310073 133 28.103 4063.103 70996.594 525.374796134 20.494 4062.357 192299.219 1423.01422 135 20.46 4046.127 45463.988336.433511 136 20.849 4044.743 40488.367 299.613916 137 28.08 4044.394166345.453 1230.95635 138 20.276 4044.247 575594.75 4259.40115 13920.865 4028.943 54097.566 400.321988 140 20.601 4025.685 273715.4382025.49424 141 28.152 4025.156 75278.781 557.062979 142 25.055 4015.313494.786 99.8614164 143 20.423 4009.552 46446.355 343.703027 144 20.884007.199 241439.844 1786.65485 145 28.076 4006.013 98433.141 728.405243146 20.719 3996.902 309862.719 2292.98412 147 20.438 3986.617 1697006.6312557.849 148 20.881 3968.808 427206.25 3161.32625 149 19.8 3960.04129275.078 956.635577 150 19.704 3913.814 25934.791 191.917453 15119.645 3900.239 29670.904 219.56469 152 19.631 3877.959 85786.75634.82195 153 19.619 3861.996 59334.113 439.072436 154 23.401 3860.22431707.752 234.637365 155 19.105 3856.541 110644.117 818.766466 15628.332 3839.987 28982.951 214.473837 157 19.659 3839.739 105607.102781.492555 158 25.36 3832.015 15375.597 113.779418 159 23.419 3822.28821333.066 157.864688 160 20.048 3814.276 379764.75 2810.25915 161 28.3733801.977 68342.133 505.731784 162 27.677 3801.896 13939.659 103.153477163 27.719 3794.861 51831.453 383.552752 164 21.453 3782.819 17585.135130.129999 165 31.428 3775.772 53642.129 396.951755 166 27.744 3772.916129047.891 954.954393 167 21.446 3760.889 121781.781 901.185179 16819.224 3760.068 42083.434 311.417412 169 21.836 3757.834 12074.3689.350264 170 27.7 3756.982 327179.375 2421.12738 171 21.886 3741.8231431.242 232.591191 172 27.715 3739.881 56333.398 416.867145 173 27.6783735.445 121638.703 900.126402 174 19.018 3729.583 19175.627 141.89964175 21.454 3722.747 1143063.38 8458.66898 176 21.905 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24.966 2483.135 101523.984 751.277482571 50.133 2480.983 6654.337 49.2420938 572 28.907 2480.171 48322.785357.588609 573 37.468 2479.164 10220.078 75.6285772 574 29.264 2471.29817940.619 132.760581 575 25.284 2468.22 27459.982 203.203867 576 53.5752466.851 50476.148 373.523495 577 55.082 2466.643 85574.617 633.252166578 28.208 2466.149 19103.148 141.363295 579 30.326 2452.741 105720.547782.332048 580 25.383 2452.241 25429.555 188.178707 581 53.558 2444.922132386.922 979.663223 582 55.038 2444.863 166593.141 1232.78924 58354.419 2443.898 14516.007 107.418452 584 28.896 2442.177 99161.281733.793479 585 47.436 2440.325 82396.445 609.733693 586 22.331 2439.34926883.18 198.935532 587 20.725 2437.156 67598.68 500.230232 588 30.3672430.738 112506.719 832.549721 589 25.309 2430.18 9069.742 67.1160908590 37.568 2430.001 10098.263 74.7271462 591 55.058 2428.844 151840.5781123.62028 592 53.565 2428.839 97552.461 721.888211 593 21.874 2427.305277859.406 2056.1596 594 28.784 2422.657 49308.391 364.882093 595 47.2642418.405 102784.953 760.608652 596 28.611 2418.047 23545.922 174.239823597 30.328 2415.783 100262.688 741.943891 598 20.7 2415.168 241525.4061787.288 599 28.755 2415.065 27699.828 204.978727 600 19.242 2414.2919697.506 145.761544 601 55.019 2411.833 8743.657 64.7030618 602 37.1192408.022 95515.813 706.817016 603 24.956 2407.143 19052.658 140.989669604 56.103 2406.969 2105.086 15.5776364 605 53.549 2406.949 105913783.7562 606 55.077 2406.902 128330.906 949.648704 607 21.91 2405.31222780.617 168.576566 608 20.28 2404.141 42368.875 313.529675 609 47.2962402.426 168612.344 1247.73135 610 20.557 2401.462 109291.289 808.755539611 28.781 2398.085 20548.543 152.059218 612 28.626 2396.215 1866261381.0324 613 54.355 2395.78 17539.246 129.79042 614 19.791 2395.3338127.117 282.140666 615 53.832 2395.108 25210.896 186.56063 616 22.1812393.58 28325.973 209.6122 617 37.389 2392.069 32789.227 242.64028 61836.842 2392.022 16480.713 121.957276 619 53.509 2390.96 7808.70557.784417 620 55.017 2390.746 56777.559 420.153937 621 21.858 2389.3671415681.5 10476.0431 622 28.783 2384.878 67750.172 501.351273 623 54.2132381.804 9437.86 69.840164 624 53.96 2379.819 13638.621 100.925795 62528.586 2379.768 179069.688 1325.11569 626 20.738 2377.238 713037.3755276.47658 627 28.792 2377.105 243979.281 1805.44668 628 54.034 2374.36998473.961 728.707311 629 38.119 2370.071 587311.313 4346.10372 63055.054 2368.829 45047.953 333.354852 631 49.833 2368.79 7574.21456.0491836 632 21.712 2364.035 14890.036 110.186266 633 47.251 2363.877169502.969 1254.32197 634 47.112 2359.46 226706.625 1677.62903 635 54.062358.796 271180 2006.732 636 28.638 2358.069 484792 3587.4608 637 30.3922356.841 24718.348 182.915775 638 49.349 2356.439 49754.129 368.180555639 22.229 2355.161 64185.695 474.974143 640 37.22 2354.086 71290.633527.550684 641 54.995 2351.738 14965.655 110.745847 642 19.26 2343.30931234.203 231.133102 643 54.345 2342.704 55254.418 408.882693 644 21.7532342.053 57971.406 428.988404 645 53.764 2341.883 102171.742 756.070891646 28.619 2341.757 395942.094 2929.9715 647 24.143 2341.072 185665.3281373.92343 648 28.832 2339.135 119528.75 884.51275 649 54.092 2336.821849316.625 6284.94303 650 49.582 2334.924 16711.031 123.661629 65149.932 2332.825 7154.382 52.9424268 652 38.111 2332.118 724905.5635364.30117 653 28.429 2332.011 26272.477 194.41633 654 49.784 2330.84818374.775 135.973335 655 20.777 2329.976 13845.191 102.454413 656 20.7812328.12 114579.438 847.887841 657 21.695 2326.051 33955.465 251.270441658 28.514 2325.829 27821.584 205.879722 659 24.109 2325.039 347883.4062574.3372 660 18.808 2323.646 3501.718 25.9127132 661 21.857 2322.10527377.75 202.59535 662 54.036 2320.85 1445477 10696.5298 663 21.7362320.083 17368.453 128.526552 664 28.756 2320.083 1394689.88 10320.7051665 31.151 2319.995 18706.303 138.426642 666 50.101 2319.65 21160.838156.590201 667 49.596 2318.781 65589.969 485.365771 668 53.96 2314.8175407.608 40.0162992 669 28.434 2313.129 21076.289 155.964539 670 20.6952312.394 183844.266 1360.44757 671 45.447 2310.83 8350.151 61.7911174672 28.377 2309.901 32903.531 243.486129 673 24.091 2309.052 53750.734397.755432 674 28.352 2308.815 65167.617 482.240366 675 19.413 2306.09311910.861 88.1403714 676 47.374 2305.43 20267.41 149.978834 677 30.4792304.938 64574.715 477.852891 678 54.005 2304.69 601818.875 4453.45968679 55.551 2304.254 20926.719 154.857721 680 28.66 2304.2 441698.6253268.56983 681 21.748 2304.056 491680.813 3638.43802 682 54.026 2298.862803671 20747.1654 683 20.539 2298.221 189552.234 1402.68653 684 30.7982295.988 10958.861 81.0955714 685 50.105 2295.884 10295.519 76.1868406686 19.179 2295.451 24928.195 184.468643 687 28.816 2295.237 260138.0161925.02132 688 28.385 2295.094 55681.145 412.040473 689 21.739 2288.10157605.777 426.28275 690 24.096 2287.057 1262872.75 9345.25835 691 28.3882287.048 297568.75 2202.00875 692 20.5 2286.111 21349.635 157.987299 69324.027 2283.095 24350.102 180.190755 694 54.068 2282.898 2728088.7520187.8568 695 28.732 2282.105 667956.938 6281.39651 4942.88134 69621.782 2282.103 58645.039 433.973289 697 30.387 2282 115145.461852.076411 698 38.199 2281.901 31642.785 234.156609 699 38.703 2281.8948948.516 66.2190184 700 40.729 2281.884 69357.18 513.243132 701 37.8472281.877 7632.981 56.4840594 702 49.628 2280.479 11230.125 83.102925 70353.207 2278.702 26455.098 195.767725 704 28.903 2273.115 293589.7192172.56392 705 28.157 2272.659 27751.025 205.357585 706 28.368 2271.091240296.203 1778.1919 707 23.951 2271.069 46381.387 343.222264 708 54.5632266.722 53080.328 392.794427 709 53.746 2266.569 194273.734 1437.62563710 21.735 2266.113 834853.813 6177.91822 711 47.142 2264.341 11589.80585.764557 712 25.004 2264.038 10342.722 76.5361428 713 54.111 2260.9063409623 25231.2102 714 39.005 2259.881 8171.715 60.470691 715 38.0182259.88 89646.383 663.383234 716 29.265 2257.021 369411.719 2733.64672717 28.144 2250.717 73907.656 546.916654 718 28.424 2249.076 762669.6885643.75569 719 20.437 2249.042 143049.578 1058.56688 720 47.446 2248.591114672.375 848.575575 721 53.175 2246.379 18363.697 135.891358 72254.105 2244.921 1221368.75 9038.12875 723 53.209 2240.749 57652.742426.630291 724 49.832 2237.759 5953.025 44.052385 725 28.924 2235.175214885.766 1590.15467 726 28.13 2234.935 156541.781 1158.40918 72728.391 2233.099 305448.406 2260.3182 728 20.474 2232.684 41022.949303.569823 729 25.029 2231.969 11965.051 88.5413774 730 23.853 2230.05138128.531 282.151129 731 25.127 2227.077 31312.469 231.712271 732 47.2532226.358 138834.063 1027.37207 733 24.982 2226.04 37025.727 273.99038734 54.067 2222.955 1451186.5 10738.7801 735 55.587 2222.909 18411.467136.244856 736 39.072 2221.946 758603.125 5613.66313 737 33.365 2221.74713675.914 101.201764 738 49.924 2221.487 22766.725 168.473765 739 28.6012216.12 62841.969 465.030571 740 21.813 2215.931 38498.379 284.888005741 28.165 2212.947 407865.344 3018.20355 742 20.541 2211.332 175885.4531301.55235 743 28.425 2211.08 604871.438 4476.04864 744 47.358 2210.38198223.844 1466.85645 745 24.99 2209.092 148361.516 1097.87522 74627.351 2208.986 43820.238 324.269761 747 34.776 2208.878 7891.0458.393696 748 23.983 2208.045 1445503.75 10696.7278 749 33.037 2207.82420242.492 149.794441 750 53.207 2207.742 5340.262 39.5179388 751 29.9612206.693 69426.469 513.755871 752 39.013 2205.963 658740.688 4874.68109753 54.008 2203.897 11335.302 83.8812348 754 53.189 2202.779 65413.605484.060677 755 19.293 2200.036 22179.658 164.129469 756 55.068 2199.7377793.02 57.668348 757 28.127 2197.011 487901.156 3610.46855 758 20.1812194.916 131013.984 969.503482 759 50.327 2194.728 41764.328 309.056027760 24.981 2193.839 73573.773 544.44592 761 20.446 2193.108 20270.781150.003779 762 54.947 2192.113 67683.648 500.858995 763 23.925 2192.015526681.563 3897.44357 764 21.89 2191.903 167538 1239.7812 765 50.8642191.723 32037.535 237.077759 766 47.244 2188.395 251956.906 1864.4811767 32.649 2188.058 78885.688 583.754091 768 24.014 2186.089 116699.281863.574679 769 29.978 2184.703 233078.734 1724.78263 770 39.09 2183.9921648277.63 12197.2544 771 50.193 2178.759 33248.797 246.041098 77254.895 2176.709 42103.77 311.567898 773 21.423 2175.984 37351.434276.400612 774 51.031 2175.813 37432.242 276.998591 775 28.214 2175.135523507.813 4308.36938 3873.95782 776 55.139 2174.695 12196.70390.2556022 777 47.254 2172.427 139909.953 1035.33365 778 24.955 2171.845392253.938 2902.67914 779 54.95 2170.835 83249.852 616.048905 780 23.992170.06 2801978.75 16950.086 20734.6428 781 33.051 2169.816 115270.117852.998866 782 28.029 2169.083 41560.289 307.546139 783 29.942 2168.74150702.242 375.196591 784 38.918 2168 625043.188 4625.31959 785 47.1052167.452 166361.109 1231.07221 786 23.628 2166.176 62101.336 459.549886787 27.877 2163.994 17963.393 132.929108 788 19.292 2163.03 26186.1193.77714 789 28.177 2159.127 165196.703 2003.94316 1222.4556 790 21.7292157.014 371334.938 2747.87854 791 50.303 2156.445 98210.313 726.756316792 24.927 2156.036 134981.219 998.861021 793 54.905 2155.728 215793.3281596.87063 794 50.291 2153.919 356736.531 2639.85033 795 33.038 2153.85317994.725 133.160965 796 24.073 2153.761 687819.375 5089.86338 79721.431 2151.975 13115.051 97.0513774 798 47.014 2150.457 80450.156595.331154 799 24.985 2150.074 124303.188 919.843591 800 23.697 2148.07814427.769 106.765491 801 47.017 2146.51 33126.008 245.132459 802 39.0312146.033 1517131 11226.7694 803 28.033 2142.049 116757.086 864.002436804 50.317 2140.053 49425.555 365.749107 805 54.907 2139.687 131492.109973.041607 806 19.34 2139.264 16454.809 121.765587 807 21.438 2138.028170402.016 1260.97492 808 49.775 2137.904 122028.063 903.007666 80951.01 2137.833 107543.789 795.824039 810 24.98 2134.064 184060.3131362.04632 811 23.947 2133.997 14915.034 110.371252 812 54.93 2133.748448603.344 3319.66475 813 23.791 2132.926 98156.297 726.356598 81433.034 2131.834 93856.258 694.536309 815 49.73 2131.826 40604.926300.476452 816 19.309 2126.895 11998.439 88.7884486 817 19.23 2125.95913855.418 102.530093 818 28.013 2125.696 179600.594 1329.0444 819 29.0332123.978 9567.942 70.8027708 820 28.424 2123.872 38521.063 285.055866821 19.288 2123.304 41390.043 306.286318 822 54.923 2117.754 676757.1255008.00273 823 50.182 2115.807 562227.938 4160.48674 824 32.559 2113.63214000.153 103.601132 825 27.977 2110.026 15948.838 118.021401 826 19.2422109.934 16406.662 121.409299 827 23.748 2108.995 14636.829 108.312535828 27.756 2106.99 38564.801 285.379527 829 20.492 2105.879 76712.156567.669954 830 54.924 2101.744 308647.25 2283.98965 831 21.456 2101.398246869.797 1826.8365 832 49.813 2099.871 64825.379 479.707805 833 50.9692099.86 21705.629 160.621655 834 22.512 2098.949 30868.66 228.428084 83554.919 2095.774 1133086.88 8384.84288 836 56.91 2094.771 16988.391125.714093 837 50.601 2094.588 22926.068 169.652903 838 23.784 2093.20675977.586 562.234136 839 28.084 2088.017 171200.609 1269.994621266.88451 840 19.264 2087.973 350660.688 2594.88909 841 23.117 2086.6512786.285 94.618509 842 27.791 2085.045 199885.375 1479.15178 843 20.2692081.018 229086.047 1695.23675 844 54.93 2079.801 993210.188 7349.75539845 47.595 2079.318 19015.662 140.715899 846 56.839 2078.89 19401.766143.573068 847 49.785 2077.893 115355.531 853.630929 848 21.811 2077.76231063.748 229.871735 849 52.075 2077.73 6613.918 48.9429932 850 21.412076.984 175348.891 1297.58179 851 51.543 2071.648 7766.515 57.472211852 23.759 2071.002 133591.328 988.575827 853 21.424 2070.003 109701.07811.787918 854 51.254 2069.625 61727.754 456.78538 855 27.817 2069.09222562.547 1646.96285 856 20.532 2067.921 477863.719 3536.19152 85727.607 2063.948 71420.422 528.511123 858 54.94 2063.804 166864.9381234.80054 859 55.581 2062.783 10409.057 77.0270218 860 22.44 2059.04531675.367 234.397716 861 54.9 2057.817 1045255.63 7734.89163 862 20.8022056.804 23316.27 172.540398 863 47.411 2056.32 114767.031 849.276029864 23.834 2056.014 75674.141 559.988643 865 52.099 2054.689 8212.41560.771871 866 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80382.313594.829116 916 27.666 1975.777 70365.492 520.704641 917 47.124 1975.433105832.047 783.157148 918 39.641 1972.397 211920.281 1568.21008 91921.264 1971.932 24054.641 178.004343 920 41.424 1971.717 16212.052119.969185 921 40.892 1971.699 25774.264 190.729554 922 51.25 1971.598203815.859 1508.23736 923 23.437 1971.004 533845.5 3950.4567 924 41.9521970.701 11751.374 86.9601676 925 49.899 1969.877 510840.781 3780.22178926 54.004 1969.775 110049.828 814.368727 927 52.803 1969.714 3832.40628.3598044 928 40.409 1967.647 566741.125 4193.88433 929 51.49 1966.7668687.899 64.2904526 930 20.143 1964.822 68999.875 510.599075 931 27.2261963.76 22017.5 162.9295 932 35.592 1961.849 215947.656 1598.01265 93320.186 1958.815 182788.188 1352.63259 934 25.235 1955.974 34034.582251.855907 935 34.906 1955.842 23583.658 174.519069 936 35.204 1954.87523046.27 170.542398 937 20.225 1954.822 104457.664 772.986714 938 27.6541954.071 25012.77 185.094498 939 49.914 1953.531 149496.656 1106.27525940 23.846 1951.907 11188.573 82.7954402 941 40.048 1951.671 405308.7812999.28498 942 49.519 1951.462 32885.328 243.351427 943 28.011 1950.92680130.508 592.965759 944 29.888 1950.847 95179.586 704.328936 945 21.3311949.954 15990.713 118.331276 946 19.872 1949.895 8138.52 60.225048 94723.457 1949.102 3147247 23289.6278 948 27.164 1947.721 65290.855483.152327 949 35.176 1945.87 48158.836 356.375386 950 51.644 1945.5335578.079 41.2777846 951 28.503 1945.117 26344.092 194.946281 952 20.191942.355 176231.625 1304.11403 953 36.009 1939.849 754929.75 5586.48015954 21.083 1939.728 83881.531 620.723329 955 27.622 1937.032 122677.93907.816682 956 20.174 1935.815 14819.995 109.667963 957 55.67 1935.5091866.308 13.8106792 958 19.929 1934.88 185292.125 1371.16173 959 27.61933.946 21970.883 162.584534 960 21.312 1933.467 120517.273 891.82782961 23.44 1933.132 1264035.38 9353.86178 962 49.882 1931.835 169525.3441254.48755 963 53.987 1931.539 7912.462 58.5522188 964 32.897 1930.83560372.492 446.756441 965 40.453 1929.642 1351748.75 10002.9408 96649.985 1928.736 30871.664 228.450314 967 19.413 1928.014 24680.447182.635308 968 22.284 1925.639 28804.176 213.150902 969 36.02 1923.804788593 5835.5882 970 32.585 1923.744 18391.229 136.095095 971 51.4741923.542 22426.631 165.957069 972 21.155 1921.892 25471.947 188.492408973 20.197 1920.513 484588.406 3585.9542 974 35.145 1917.819 151947.5471124.41185 975 20.275 1916.865 592958 4387.8892 976 32.944 1914.8553011.285 392.283509 977 39.532 1913.055 359803.531 2662.54613 97827.873 1912.956 171374.188 1268.16899 979 49.886 1912.77 90604.273670.47162 980 23.536 1911.131 16659075 123277.155 981 19.165 1909.16916568.082 122.603807 982 35.112 1907.913 132959.188 983.897991 983 51.451907.405 55725.84 412.371216 984 20.208 1904.837 417636.094 3090.5071985 19.974 1901.937 12937.851 95.7400974 986 36.035 1901.931 1493067.8811048.7023 987 27.44 1901.067 35484.109 262.582407 988 21.174 1898.89249621.984 367.202682 989 26.836 1897.634 51880.426 383.915152 990 22.5691895.801 31370.744 232.143506 991 50.839 1895.655 14071.792 104.131261992 19.364 1893.904 10081.896 74.6060304 993 20.096 1893.708 16126.631119.337069 994 23.44 1893.144 138012.906 1021.2955 995 33.628 1892.875666429.375 4931.57738 996 40.178 1891.728 965003.063 7141.02267 99723.747 1890.939 199265.828 1474.56713 998 28.18 1889.913 10303.56576.246381 999 51.81 1886.097 32181.391 238.142293 1000 49.855 1886.0179415.063 69.6714662 1001 19.928 1885.96 15694.74 116.141076 1002 35.931885.943 758995.75 5616.56855 1003 51.337 1885.571 114489.086 847.2192361004 20.18 1882.925 4423241 32731.9834 1005 29.37 1882.543 68798.625509.109825 1006 35.135 1879.95 58723.824 434.556298 1007 22.494 1879.25720705.602 153.221455 1008 34.349 1878.875 33668.203 249.144702 100922.591 1876.914 37062.238 274.260561 1010 21.725 1876.902 297599.3131550.63508 2202.23492 1011 32.986 1876.876 128455.727 950.57238 101255.924 1875.624 2100.854 15.5463196 1013 26.625 1875.501 105028.836777.213386 1014 27.296 1874.767 67852.57 502.109018 1015 26.891 1873.89193489.258 691.820509 1016 21.431 1872.932 23245.711 172.018261 101719.83 1872.86 146425.875 1083.55148 1018 51.282 1869.592 141043.2341043.71993 1019 20.63 1867.838 31031.188 229.630791 1020 27.992 1864.67533520.336 248.050486 1021 47.391 1864.278 57918.516 428.597018 102220.099 1864.101 137271.891 1015.81199 1023 35.869 1863.967 524659.4383882.47984 1024 27.239 1863.873 52788.363 390.633886 1025 20.0311863.141 139697.438 1033.76104 1026 19.87 1860.926 13068.771 96.70890541027 21.157 1860.926 81917.836 606.191986 1028 26.764 1860.34 197601.5311462.25133 1029 27.282 1859.5 48407.289 358.213939 1030 23.006 1859.03193516.188 1432.01979 1031 51.461 1858.652 43128.02 319.147348 103222.605 1857.839 203838.828 1508.40733 1033 19.267 1855.928 13138.12697.2221324 1034 20.105 1855.764 131766.063 975.068866 1035 33.5771854.908 733231.875 5425.91588 1036 26.818 1851.8 200711.625 1485.266031037 60.637 1848.46 6038.243 44.6829982 1038 19.998 1848.263 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55.5830576 1690 30.98 1401.473171155.313 1266.54932 1691 25.705 1400.678 71240.352 527.178605 169260.454 1399.435 15121.45 111.89873 1693 19.068 1397.692 3839.19928.4100726 1694 25.389 1397.57 528235.875 3908.94548 1695 32.2881396.606 10441.645 77.268173 1696 31.138 1396.434 127553.898 943.8988451697 57.725 1396.36 55281.977 409.08663 1698 21.421 1392.695 709464.3135250.03592 1699 59.374 1391.448 4601.684 34.0524616 1700 59.651 1391.4282721.883 20.1419342 1701 45.062 1390.986 37551.5 277.8811 1702 31.0911390.532 1131354.75 8372.02515 1703 32.449 1389.93 406237.781 3006.159581704 43.567 1388.482 94132.688 696.581891 1705 51.546 1386.784 3704.04927.4099626 1706 25.04 1386.521 93427.875 691.366275 1707 59.273 1386.3624964.27 184.735598 1708 45.063 1385.978 210238.953 1555.76825 170951.138 1385.566 41882.465 309.930241 1710 30.901 1385.488 20099.48148.736152 1711 59.7 1382.403 30916.771 228.784105 1712 47.077 1382.27364972.203 480.794302 1713 25.349 1381.698 426013.25 3152.49805 171421.186 1380.693 20415.264 151.072954 1715 25.109 1380.547 10967.78181.1615794 1716 53.108 1380.342 13301.506 98.4311444 1717 25.6791378.704 342898.781 2415.39444 2537.45098 1718 49.632 1378.394 5379.27439.8066276 1719 18.97 1377.85 30348.645 224.579973 1720 25.346 1375.62446687.473 345.4873 1721 32.125 1375.532 67528.18 499.708532 1722 37.3691375.445 8201.093 60.6880882 1723 34.801 1375.438 17825.877 131.911491724 55.31 1374.42 31385.559 232.253137 1725 56.785 1374.415 9927.62373.4644102 1726 32.405 1373.689 38635.266 285.900968 1727 60.227 1373.366000.033 44.4002442 1728 45.05 1368.949 34093.426 252.291352 1729 32.4641367.728 132403.016 979.782318 1730 55.22 1367.496 1103.651 8.16701741731 60.375 1366.465 12431.157 91.9905618 1732 25.359 1365.647 47731.473353.2129 1733 45.052 1365.037 104198.375 771.067975 1734 19.189 1364.74811513.005 85.196237 1735 25.813 1364.605 75452.961 558.351911 173625.024 1364.429 298666.156 2210.12955 1737 51.066 1363.59 4498.99933.2925926 1738 30.979 1363.458 95695.992 708.150341 1739 45.02 1362.89110947.891 821.014393 1740 32.068 1359.662 52750.859 390.356357 174125.534 1359.656 1906445.75 14107.6986 1742 31.049 1358.466 151038.2811117.68328 1743 49.608 1356.381 45604.996 337.47697 1744 59.708 1356.31929863.813 220.992216 1745 60.659 1355.61 1210.575 8.958255 1746 55.5721354.558 1049.276 7.7646424 1747 58.894 1354.391 2738.662 20.26609881748 23.999 1353.72 101441.016 750.663518 1749 23.416 1352.847 43856.227324.53608 1750 30.605 1352.398 90038.555 666.285307 1751 32.39 1351.68632230.543 238.506018 1752 34.799 1351.387 8059.731 59.6420094 175325.989 1350.605 40075.652 296.559825 1754 59.605 1350.549 6613.85448.9425196 1755 59.372 1349.363 5556.154 41.1155396 1756 25.073 1348.535290868.375 2152.42598 1757 18.811 1347.718 12626.824 93.4384976 175825.458 1343.664 766104.375 5669.17238 1759 26.465 1342.628 17343.17128.339458 1760 53.156 1342.392 5754.031 42.5798294 1761 45.041 1341.946191931.266 1420.29137 1762 29.936 1339.384 45313.438 335.319441 176322.748 1338.66 77636.578 574.510677 1764 60.353 1338.395 2928.56421.6713736 1765 30.621 1336.417 37646.219 278.582021 1766 55.0911334.981 17385.801 128.654927 1767 59.445 1334.35 36656.449 271.2577231768 19.066 1332.751 11472.639 84.8975286 1769 25.099 1332.551113287.906 838.330504 1770 59.549 1330.309 2890.745 21.391513 177159.275 1330.277 9237.706 68.3590244 1772 25.154 1326.551 949441.6257025.86803 1773 45.045 1324.926 42727.93 316.186682 1774 31.961 1322.60328099.598 207.937025 1775 25.586 1321.685 2478338.5 18339.7049 177630.808 1321.321 58397.359 432.140457 1777 45.004 1321.021 66336.734490.891832 1778 20.636 1320.662 25817.596 191.05021 1779 32.429 1319.44111738.492 86.8648408 1780 31.4 1319.42 6886.302 50.9586348 1781 52.9541319.408 3111.002 23.0214148 1782 50.24 1319.394 4092.932 30.28769681783 48.515 1319.389 12137.362 89.8164788 1784 34.136 1319.387 43983.848325.480475 1785 35.227 1319.362 4880.322 36.1143828 1786 45 1318.86187233.422 645.527323 1787 31.907 1318.611 13398.739 99.1506686 178841.768 1318.589 232563.891 1720.97279 1789 39.529 1318.407 9566.11370.7892362 1790 46.954 1318.405 13212.546 97.7728404 1791 53.1541318.387 4069.485 30.114189 1792 39.074 1318.375 7447.503 55.11152221793 59.704 1318.363 36163.148 267.607295 1794 30.603 1314.452239448.859 1771.92156 1795 21.917 1312.679 77039.18 570.089932 179626.005 1312.635 141686.484 1048.47998 1797 52.047 1311.498 829.6176.1391658 1798 25.103 1310.563 660235.938 4885.74594 1799 60.2271306.401 3903.396 28.8851304 1800 45.07 1303.966 34127.25 252.54165 180125.985 1302.62 19980.832 147.858157 1802 51.644 1302.438 2354.19317.4210282 1803 59.746 1302.393 45806.871 338.970845 1804 22.2521301.272 57392.363 424.703486 1805 54.153 1300.353 8612.625 63.7334251806 21.95 1299.873 83524.633 618.082284 1807 51.573 1299.424 30573.758226.245809 1808 53.107 1299.416 25302.227 187.23648 1809 19.258 1298.64221156.547 156.558448 1810 59.374 1298.359 12482.001 92.3668074 181145.03 1297.919 185944.781 1375.99138 1812 19.022 1296.685 28328.535209.631159 1813 59.676 1295.779 9187.956 67.9908744 1814 28.449 1295.485170789.578 1263.84288 1815 25.008 1294.604 46179.98 341.731852 181630.249 1293.53 103213.75 763.78175 1817 23.194 1292.502 19937.287147.535924 1818 30.646 1290.433 8808.077 65.1797698 1819 28.43 1289.45618305.74 135.462476 1820 58.946 1289.403 1384.637 10.2463138 1821 59.6271289.387 2301.153 17.0285322 1822 19.693 1289.386 4377.44 32.393056 182325.244 1288.534 2999592.25 22196.9827 1824 59.353 1286.338 15882.02117.526948 1825 30.82 1283.472 39585.328 292.931427 1826 51.523 1283.4456039.294 44.6907756 1827 53.186 1283.43 8806.266 65.1663684 1828 34.8021283.335 8705.754 64.4225796 1829 59.03 1282.394 15341.116 113.5242581830 55.529 1282.378 7111.861 52.6277714 1831 45.022 1280.883 30969.486229.174196 1832 19.518 1280.665 11716.79 86.704246 1833 59.668 1280.41149052 362.9848 1834 28.452 1279.513 51832.395 383.559723 1835 51.441277.454 82467.625 610.260425 1836 52.927 1277.446 43342.348 320.7333751837 45.003 1276.982 70758.93 523.616082 1838 30.44 1276.942 232610.751721.31955 1839 50.608 1276.907 1109.392 8.2095008 1840 23.116 1276.515122081.953 903.406452 1841 44.995 1274.825 81134.063 600.392066 184226.295 1272.61 41668.891 308.349793 1843 25.135 1272.604 1010380.887476.81848 1844 20.731 1272.48 34951.859 258.643757 1845 30.456 1272.332289698.906 2143.7719 1846 31.95 1270.569 58033.617 429.448766 184754.813 1270.498 1479.774 10.9503276 1848 59.96 1270.475 3445.86625.4994084 1849 57.989 1270.447 1281.669 9.4843506 1850 59.188 1270.4245638.458 41.7245892 1851 37.091 1269.475 1353.805 10.018157 1852 40.971269.437 2427.428 17.9629672 1853 35.834 1269.418 2728.887 20.19376381854 40.087 1269.413 1651.728 12.2227872 1855 39.127 1269.409 5886.62243.5610028 1856 36.13 1269.399 4146.72 30.685728 1857 30.571 1267.51521216.277 157.00045 1858 59.349 1266.399 6219.467 46.0240558 1859 54.8941266.362 4477.317 33.1321458 1860 22.184 1263.606 94234.227 697.333281861 59.935 1263.437 57252.406 423.667804 1862 34.938 1263.312 16850.229124.691695 1863 37.489 1262.942 10585.427 78.3321598 1864 55.3421262.696 14468.394 107.066116 1865 52.525 1262.35 8346.335 61.7628791866 39.287 1262.338 12846.079 95.0609846 1867 40.214 1262.335 8975.61866.4195732 1868 58.04 1262.315 3522.354 26.0654196 1869 21.765 1262.289123903.367 916.884916 1870 51.525 1261.458 99836.336 738.788886 187153.043 1261.455 83416.992 617.285741 1872 23.116 1260.537 46480.016343.952118 1873 34.799 1259.311 14362.161 106.279991 1874 28.4591257.534 298317.219 2207.54742 1875 31.559 1255.699 116446.039861.700689 1876 30.3 1255.583 846248.25 6262.23705 1877 32.837 1255.56735492.637 262.645514 1878 33.291 1255.561 28837.1 213.39454 1879 51.2441255.489 2861.904 21.1780896 1880 32.024 1254.973 95395.18 705.9243321881 23.278 1254.568 121895.391 902.025893 1882 59.74 1254.366 5949.09544.023303 1883 57.787 1254.364 4684.266 34.6635684 1884 58.949 1254.3472524.573 18.6818402 1885 57.081 1254.319 8885.642 65.7537508 1886 55.4211254.301 4541.622 33.6080028 1887 45.012 1253.896 147699.641 1092.977341888 28.407 1251.496 141158.859 1044.57556 1889 25.249 1250.6313974873.75 34371.53 29414.0658 1890 58.643 1250.455 11072.911 81.93954141891 18.98 1249.756 27491.875 203.439875 1892 31.656 1248.538 26623.307197.012472 1893 32.92 1247.361 41003.309 303.424487 1894 51.498 1245.4988761.765 64.837061 1895 53.085 1245.476 44366.938 328.315341 1896 19.6321244.64 30831.113 228.150236 1897 59.714 1242.427 56404.984 417.3968821898 56.779 1241.078 2758.177 20.4105098 1899 30.278 1239.607 317820.0632351.86847 1900 31.547 1239.563 59098.148 437.326295 1901 28.4721239.526 69276.641 512.647143 1902 51.321 1239.492 69059.977 511.043831903 52.866 1239.474 32897.426 243.440952 1904 60.102 1238.604 6424.09147.5382734 1905 23.198 1238.572 492393.188 3643.70959 1906 25.0571238.532 9391.734 69.4988316 1907 37.49 1237.332 6531.968 48.33656321908 45.022 1236.87 46682.961 345.453911 1909 19.717 1236.611 7412.52454.8526776 1910 40.236 1236.283 8209.991 60.7539334 1911 52.172 1235.898888.905 6.577897 1912 19.301 1235.868 4725.906 34.9717044 1913 30.4171234.37 856949.25 6341.42445 1914 31.611 1233.532 122064.055 903.2740071915 25.133 1232.595 24227.906 179.286504 1916 21.214 1231.482 60734.938449.438541 1917 32.839 1231.084 60950.719 451.035321 1918 42.8551230.887 154045.125 1139.93393 1919 30.565 1229.563 91573.625 677.6448251920 22.209 1228.627 18700.881 138.386519 1921 60.379 1227.376 3367.17624.9171024 1922 52.522 1227.324 6150.93 45.516882 1923 51.79 1227.3234718.815 34.919231 1924 49.813 1227.305 11513.576 85.2004624 1925 40.1921227.301 7194.075 53.236155 1926 59.636 1226.901 24848.395 183.8781231927 21.859 1224.549 44181.957 326.946482 1928 30.406 1224.415 69779.727516.36998 1929 23.094 1222.581 91712.016 678.668918 1930 51.595 1222.4713662.568 27.1030032 1931 30.29 1218.52 476128.844 3523.35345 1932 31.5281217.669 163110.922 1207.02082 1933 25.119 1217.539 169168.7341251.84863 1934 23.259 1216.597 263113.625 1947.04083 1935 44.9961215.355 16854.1 124.72034 1936 31.638 1211.447 117543.125 869.8191251937 55.57 1210.742 2894.646 21.4203804 1938 20.68 1210.615 33522.359248.065457 1939 31.023 1210.478 47086.57 348.440618 1940 60.002 1210.3782460.045 18.204333 1941 59.452 1210.36 2822.82 20.888868 1942 53.3671210.321 12792.264 94.6627536 1943 56.782 1210.2 4122.384 30.50564161944 45.004 1209.865 121766.766 901.074068 1945 25.804 1209.47 31311.213231.702976 1946 20.729 1206.596 10410.285 77.036109 1947 51.214 1205.4913944.53 29.189522 1948 31.553 1203.616 23597.301 174.620027 1949 49.5161203.133 8821.522 65.2792628 1950 30.195 1202.589 39710.629 293.8586551951 50.689 1202.365 25647.943 189.794778 1952 51.135 1201.518 6787.76950.2294906 1953 42.67 1200.783 72117.422 533.668923 1954 23.167 1200.6091313535.88 9720.16548 1955 25.206 1200.547 16658.26 123.271124 195646.71 1200.503 19274.873 142.63406 1957 30.044 1198.562 22444.525166.089485 1958 59.87 1198.361 4803.752 35.5477648 1959 59.432 1198.3534145.694 30.6781356 1960 19.706 1198.222 12631.365 93.472101 1961 21.0131197.031 87272.023 645.81297 1962 30.406 1196.417 620780.5 4593.77571963 60.6 1196.352 7650.589 56.6143586 1964 31.578 1195.579 464075.1883434.15639 1965 59.222 1190.363 5847.735 43.273239 1966 53.252 1188.33455063.84 407.472416 1967 59.825 1187.418 3255.71 24.092254 1968 21.8821186.597 192521.25 1424.65725 1969 60.255 1186.382 6004.868 44.43602321970 30.174 1185.657 58927.867 436.066216 1971 42.453 1184.524 53516.508396.022159 1972 59.174 1184.402 4914.623 36.3682102 1973 21.325 1183.635234638.141 1736.32224 1974 59.7 1183.443 7250.531 53.6539294 1975 31.8011182.586 11399.009 84.3526666 1976 31.299 1181.569 94998.031 702.9854291977 49.745 1181.254 3827.925 28.326645 1978 56.778 1181.221 3641.41726.9464858 1979 60.62 1180.368 5690.042 42.1063108 1980 50.733 1180.33538225.785 282.870809 1981 31.583 1179.597 236420.203 1749.5095 198219.143 1178.579 11057.592 81.8261808 1983 20.779 1178.495 131686.141974.477443 1984 51.247 1178.431 6476.849 47.9286826 1985 41.654 1178.3976623.212 49.0117688 1986 56.782 1178.216 4255.032 31.4872368 1987 25.3331175.511 22551.197 166.878858 1988 24.101 1172.463 51734.363 382.8342861989 53.214 1172.348 38737.391 286.656693 1990 44.949 1170.829 10637.76978.7194906 1991 22.67 1169.26 18541.186 137.204776 1992 54.977 1169.1677155.165 52.948221 1993 60.253 1166.411 2237.358 16.5564492 1994 53.221166.339 140311.391 1038.30429 1995 31.322 1165.301 58614.336 433.7460861996 31.542 1163.587 34373.684 254.365262 1997 42.864 1163.561317640.313 2350.53832 1998 20.221 1162.602 72301.289 535.029539 199930.294 1160.457 18931.172 140.090673 2000 20.533 1159.644 11926.85488.2587196 2001 25.361 1158.633 29713.969 219.883371 2002 31.5291157.615 44626.973 330.2396 2003 24.123 1156.492 33221.211 245.8369612004 19.431 1154.638 47105.656 348.581854 2005 31.311 1154.523 72400.438535.763241 2006 23.924 1152.527 201380.953 1490.21905 2007 30.3841152.393 58578.801 433.483127 2008 21.985 1150.625 37468.707 277.2684322009 53.194 1150.361 120706.516 893.228218 2010 30.027 1149.312119640.453 885.339352 2011 42.541 1147.575 30441.695 225.268543 201223.629 1144.649 29225.717 216.270306 2013 31.311 1143.136 23237.896171.96043 2014 24.001 1142.545 23198.781 171.670979 2015 50.597 1142.373118697.242 878.359591 2016 23.275 1141.59 47004.074 347.830148 201721.014 1140.488 174479.281 1291.14668 2018 41.649 1140.415 5001.42937.0105746 2019 19.442 1138.647 71437.797 528.639698 2020 31.3671138.553 111894.984 828.022882 2021 25.359 1137.454 68654.234 508.0413322022 53.625 1137.364 4344.629 32.1502546 2023 23.802 1136.534 21588.393159.754108 2024 25.107 1135.542 37640.664 278.540914 2025 22.9041134.648 71461.75 528.81695 2026 24.113 1134.504 347155.5 2568.9507 202760.091 1134.459 5499.415 40.695671 2028 59.353 1134.437 3032.86522.443201 2029 53.188 1134.391 56996.746 421.77592 2030 51.575 1134.219499.726 70.2979724 2031 29.971 1133.34 41626.363 308.035086 2032 20.9361128.605 47002.93 347.821682 2033 28.199 1128.485 105328.227 779.428882034 53.209 1128.38 354067.813 2620.10182 2035 50.589 1126.389 28851.957213.504482 2036 31.552 1125.231 11812.239 87.4105686 2037 41.8681125.221 15596.393 115.413308 2038 32.903 1125.218 126022.156 932.5639542039 31.908 1125.217 25750.453 190.553352 2040 39.864 1125.21 6728.26449.7891536 2041 36.571 1125.206 22293.379 164.971005 2042 39.5561125.202 16396.361 121.333071 2043 26.016 1125.161 31188 230.7912 204429.167 1125.148 41243.914 305.204964 2045 38.059 1124.829 29475.412218.118049 2046 31.341 1122.552 34561.762 255.757039 2047 23.72 1122.45636783.59 272.198566 2048 44.964 1121.808 44746.047 331.120748 204918.812 1119.758 5198.635 38.469899 2050 24.134 1118.525 119093.102881.288955 2051 25.151 1118.499 30842.926 228.237652 2052 23.8991114.554 208412.047 1542.24915 2053 29.989 1111.346 183555.8911358.31359 2054 28.181 1110.479 70840.586 524.220336 2055 51.1471110.414 125425.094 928.145696 2056 20.151 1108.578 25817.43 191.0489822057 23.801 1106.903 187048.984 1384.16248 2058 50.557 1104.421171816.922 1271.44522 2059 58.615 1102.375 6383.561 47.2383514 206051.593 1101.214 1985.06 14.689444 2061 49.777 1100.828 2256.38916.6972786 2062 19.219 1100.543 6005.286 44.4391164 2063 21.831 1100.52238794.496 287.07927 2064 25.329 1099.552 13957.11 103.282614 2065 53.5451099.417 30059.629 222.441255 2066 21.401 1098.745 112194.32 830.2379682067 52.17 1098.418 3632.612 26.8813288 2068 20.123 1097.551 4589.07133.9591254 2069 24.128 1096.552 522675.844 3867.80125 2070 53.2851096.434 26559.404 196.53959 2071 51.387 1096.263 109630.906 811.2687042072 29.987 1095.392 58529 433.1146 2073 19.018 1094.643 6701.29349.5895682 2074 20.501 1091.546 15707.116 116.232658 2075 23.5981090.488 10901.328 80.6698272 2076 53.19 1090.433 338706.531 2506.428332077 20.982 1082.62 65489.449 484.621923 2078 21.397 1082.584 32035.098237.059725 2079 19.289 1080.554 12653.619 93.6367806 2080 53.4081076.445 4457.142 32.9828508 2081 53.657 1076.436 3256.97 24.101578 208252.905 1076.431 2378.771 17.6029054 2083 20.569 1075.555 86250.758638.255609 2084 29.991 1073.413 40851.953 302.304452 2085 23.4941068.813 147886.688 1094.36149 2086 21.443 1068.575 62297.086 460.9984362087 18.988 1068.472 18219.826 134.826712 2088 23.8 1064.568 7053.47552.195715 2089 20.279 1063.503 21330.266 157.843968 2090 19.116 1062.6634397.519 32.5416406 2091 32.024 1060.467 45340.27 335.517998 2092 60.6031060.416 6794.908 50.2823192 2093 52.255 1058.393 12166.359 90.03105662094 54.069 1058.366 9593.294 70.9903756 2095 49.741 1057.321 5347.42139.5709154 2096 23.962 1054.469 82210.703 608.359202 2097 23.5881051.388 89102.742 659.360291 2098 30.345 1044.353 4195.99 31.0503262099 23.401 1040.537 10620.867 78.5944158 2100 20.577 1032.597 21339.391157.911493 2101 24.092 1025.286 62953.594 465.856596 2102 19.87 1018.5277472.115 55.293651 2103 23.953 1016.515 121646.805 900.186357 210430.418 1016.354 134689.156 996.699754 2105 20.528 1015.594 21665.502160.324715 2106 23.573 1013.438 115542.805 855.016757 2107 30.3921011.276 33455.215 247.568591 2108 18.922 1010.399 9148.562 67.69935882109 20.423 1006.679 8503.45 62.92553 2110 47.1 998.211 46778.898346.163845 2111 23.462 995.402 32905.055 243.497407 2112 51.388 991.2142437.004 18.0338296 2113 21.942 988.585 32196.633 238.255084 2114 20.878988.565 12280.876 90.8784824 2115 29.367 987.262 48744.594 360.7099962116 23.484 984.509 27134.879 200.798105 2117 47.966 984.342 3780.82827.9781272 2118 23.398 981.665 20057.672 148.426773 2119 30.895 981.50225569.025 189.210785 2120 19.773 978.532 4305.65 31.86181 2121 30.386973.323 32013.334 236.898672 2122 29.291 971.253 5491.579 40.63768462123 20.901 969.104 41305.473 305.6605 2124 25.141 965.491 48757.68360.806832 2125 24.072 964.44 7556.274 55.9164276 2126 20.829 963.20616317.524 120.749678 2127 28.81 962.49 19231.721 142.314735 2128 20.219960.462 9783.454 72.3975596 2129 23.379 956.597 24888.623 184.17581 213022.899 956.484 12570.926 93.0248524 2131 59.245 955.564 1391.34310.2959382 2132 19.095 954.938 8325.797 61.6108978 2133 20.123 952.4945814.21 43.025154 2134 60.591 950.571 4099.453 30.3359522 2135 40.291950.357 19953.055 147.652607 2136 41.194 950.357 47130.363 348.7646862137 24.004 949.406 63025.402 466.387975 2138 29.386 949.317 56691.895419.520023 2139 51.536 948.37 24475.225 181.116665 2140 60.327 947.6394107.147 30.3928878 2141 23.951 945.481 43559.406 322.339604 2142 20.894944.588 148397.719 1098.14312 2143 30.047 944.458 13261.684 98.13646162144 23.976 933.488 10559.713 78.1418762 2145 20.085 931.546 45600.914337.446764 2146 18.961 926.553 4596.708 34.0156392 2147 20.898 925.26449014.879 362.710105 2148 20.978 920.557 5005.199 37.0384726 2149 18.938918.591 4865.919 36.0078006 2150 56.883 918.079 1112.862 8.2351788 215151.665 915.677 1583.223 11.7158502 2152 52.923 915.395 2432.00517.996837 2153 29.904 914.917 25552.555 189.088907 2154 40.82 912.413454771.625 3365.31003 2155 23.975 911.5 11979.838 88.6508012 2156 18.986911.287 4659.146 34.4776804 2157 29.339 906.271 22190.25 164.20785 215851.09 902.979 700.182 5.1813468 2159 20.832 902.486 52433.75 388.009752160 49.645 900.36 24044.1 177.92634 2161 24.096 898.383 45429.156336.175754 2162 56.504 897.659 5498.265 40.687161 2163 56.278 896.8291467.63 10.860462 2164 22.577 896.41 21323.018 157.790333 2165 19.262895.584 4205.946 31.1240004 2166 23.992 882.405 17175.494 127.0986562167 55.786 880.774 2373.386 17.5630564 2168 59.474 879.635 1745.67512.917995 2169 19.949 879.567 5377.363 39.7924862 2170 29.754 876.47323381.605 173.023877 2171 42.753 875.379 114573.516 847.844018 217221.028 872.459 5747.54 42.531796 2173 19.956 868.588 5911.415 43.7444712174 51.593 867.774 1445.617 10.6975658 2175 55.321 867.675 724.9745.3648076 2176 59.198 867.635 1190.664 8.8109136 2177 58.799 867.6222502.561 18.5189514 2178 20.829 852.468 7367.667 54.5207358 2179 49.047846.946 1713.276 12.6782424 2180 57.438 846.946 2112.215 15.630391 218160.566 846.924 2585.42 19.132108 2182 22.644 846.426 1215.356 8.99363442183 29.086 841.303 8721.339 64.5379086 2184 53.187 837.301 11143.63882.4629212 2185 55.22 835.737 611.264 4.5233536 2186 54.381 832.2531154.893 8.5462082 2187 59.347 824.672 836.045 6.186733 2188 20.776824.421 2193.866 16.2346084 2189 59.758 824.025 5333.992 39.4715408 219058.792 823.646 7006.314 51.8467236 2191 53.249 821.319 3106.75122.9899574 2192 60.055 815.685 1288.741 9.5366834 2193 29.084 815.4162310.018 17.0941332 2194 50.654 813.317 13369.253 98.9324722 2195 53.192799.334 37386.438 276.659641The quality of the regression is shown in FIG. 2.

1. A process for normalizing the concentration of at least one analytein a urine sample, comprising the following steps: a) associating atleast a portion of the urine sample with an analytical instrument todetermine the concentration of at least one analyte in the sample; b)associating at least a portion of the urine sample with an analyticalinstrument to determine the concentration of at least one collagen orcollagen fragment within the sample, wherein the determining of theconcentration of the at least one collagen or collagen fragmentcomprises 1) separating at least one collagen or collagen fragments fromthe sample or a portion thereof; 2) performing mass spectrometry; orusing a combination of 1) and 2); and c) normalizing the concentrationof said at least one analyte relative to the concentration of said atleast one collagen or collagen fragment.
 2. The process according toclaim 1, wherein the urine sample is subdivided by separation intoseveral subsamples before the concentration of the analyte isdetermined.
 3. The process according to claim 2, wherein said separationis effected by: chromatographic methods, adsorption to specificmaterials, or electrophoretic methods.
 4. The process according to claim1, wherein said determination of the concentration of analytes and/orcollagen or collagen fragments is effected by a UV/Vis detector,fluorescence detector, refractive index detector, diode array detector,mass spectrometer, or gel scanner.
 5. The process according to claim 1,wherein said at least one collagen or collagen fragment is identified byits migration or retention time and optionally further suitableparameters including mass spectra, UV/Vis spectra, fluorescence spectra,or affinity for particular ligands including antibodies.
 6. The processaccording to claim 1, wherein said at least one collagen fragment isselected from the peptides of SEQ ID Nos. 1 to
 42. 7. The processaccording to claim 1, wherein the concentrations of at least twocollagens or collagen fragments are determined and employed fornormalization.
 8. The process according to claim 1, wherein saidnormalization is effected by using a linear regression established withcollagen protein standards.
 9. The process according to claim 3, whereinthe said chromatographic methods is affinity chromatography,ion-exchange chromatography, reversed-phase chromatography, hydrophobicinteraction chromatography, or gel filtration.
 10. The process accordingto claim 3, wherein said chromatographic methods use FPLC or HPLC. 11.The process according to claim 3, wherein said adsorption to specificmaterial is effected by a SELDI process or a ClinProt process.
 12. Theprocess according to claim 2, wherein said separation is effected by gelelectrophoresis or capillary electrophoresis.
 13. The process accordingto claim 1, wherein the analytes and/or collagen or collagen fragmentswere treated with staining or derivatization prior to the determinationsteps.
 14. The process according to claim 5, wherein the collagen orcollagen fragment is further identified by parameters obtained by massspectra, UV/Vis spectra, fluorescence spectra, or affinity forparticular ligands.
 15. The process according to claim 1, wherein theconcentrations of at least 5 collagens or collagen fragments aredetermined and employed for normalization.
 16. The process according toclaim 1, wherein the concentrations of at least 30 collagens or collagenfragments are determined and employed for normalization.
 17. The processaccording to claim 1, wherein the concentrations of at least 50collagens or collagen fragments are determined and employed fornormalization.